CCS ChemistryPub Date : 2024-04-18DOI: 10.31635/ccschem.024.202404056
Tamara Rodríguez-Prieto, Darren Wragg, Nicole Heiduk, Mihyun Park, Nicole Strittmatter, Roland A. Fischer, Angela Casini, Guillermo Moreno-Alcántar
{"title":"A Golden Touch in the Design of Multifunctional Porphyrin Metallacages: Host–Guest Chemistry for Drug-Target Interactions","authors":"Tamara Rodríguez-Prieto, Darren Wragg, Nicole Heiduk, Mihyun Park, Nicole Strittmatter, Roland A. Fischer, Angela Casini, Guillermo Moreno-Alcántar","doi":"10.31635/ccschem.024.202404056","DOIUrl":"https://doi.org/10.31635/ccschem.024.202404056","url":null,"abstract":"<p>The use of three-dimensional self-assembled metallacages (MCgs) as multimodal drug platforms holds great promise. However, the synthesis of MCgs with increased complexity and functionality is a great challenge since understanding of the interaction of MCgs with biological targets is still limited. In this context, this work reports on the integration of a gold(III) porphyrin scaffold into a prismatic MCg structure and explores its application for multimodal therapy of cancer in vitro, namely enabling both photodynamic therapy and chemotherapy. Combining experimental approaches with a state-of-the-art metadynamics theoretical study, we discovered that the gold cage shows unprecedented host–guest interaction-driven selective stabilization of guanine-quadruplex (G4) structures – validated anticancer drug targets – disclosing a new mechanism to pursue in the design of supramolecular drugs.</p>","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":null,"pages":null},"PeriodicalIF":11.2,"publicationDate":"2024-04-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140620543","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
CCS ChemistryPub Date : 2024-04-17DOI: 10.31635/ccschem.024.202404142
Yang Feng, Zhenheng Huang, Ruochen Zhang, Beidou Zhong, Zhonghan Wu, Yanpeng Fan, Zhenhua Yan, Kai Zhang, Jun Chen
{"title":"A Quasi-Solid-State Electrolyte with Semi-Immobilized Solvent-Like Sites for Lithium-Metal Batteries","authors":"Yang Feng, Zhenheng Huang, Ruochen Zhang, Beidou Zhong, Zhonghan Wu, Yanpeng Fan, Zhenhua Yan, Kai Zhang, Jun Chen","doi":"10.31635/ccschem.024.202404142","DOIUrl":"https://doi.org/10.31635/ccschem.024.202404142","url":null,"abstract":"Quasi solid-state lithium-metal batteries (QSSLMBs) hold significant promise for enhanced energy density when compared to conventional battery systems. Nevertheless, current QSSLMBs face challenges in lithium dendrites and electrode-electrolyte interfacial side reactions driven by excessive active free solvent molecules. Herein, a metal-organic framework (MOF) with chemically grafted soft multi-ether molecules (D-Gluconic acid,2,4:3,5-di-O-methylene-, denoted as G) has been proposed to serve as a solid-state electrolyte (SSE). The as-obtained MOF-G-based electrolyte (MGE) comprises structured MOF channels with semi-immobilized solvent-like sites (G molecules), which replace liquid molecules to coordinate with Li<sup>+</sup> ions. The MGE reduces the demand for solvents compared with traditional QSSEs, thus suppressing interface side reactions. This arrangement also facilitates achieving an elevated Li<sup>+</sup> transference number (0.64) and a broad electrochemical stability window (5.4 V). Ultimately, the solid-state Li//Li symmetrical battery displays an extended lifetime surpassing 1500 h under 1 mA cm<sup>−2</sup>. The solid-state LiFePO4//Li battery utilizing the flame retarded MGE attains an impressive capacity retention of 95.75% over 600 cycles. The MOF-based functionalization strategy introduces an innovative approach to designing high-performance SSE for the advanced solid-state LMBs.\u0000<figure><img alt=\"\" data-lg-src=\"/cms/asset/44463887-8f67-463e-afbf-25ad1cf600fa/keyimage.jpg\" data-src=\"/cms/asset/af2fc54c-82f4-473d-9df4-5948ffe19c1b/keyimage.jpg\" src=\"/specs/ux3/releasedAssets/images/loader-7e60691fbe777356dc81ff6d223a82a6.gif\"/><ul>\u0000<li>Download figure</li>\u0000<li>Download PowerPoint</li>\u0000</ul>\u0000</figure>","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":null,"pages":null},"PeriodicalIF":11.2,"publicationDate":"2024-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140603935","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
CCS ChemistryPub Date : 2024-04-17DOI: 10.31635/ccschem.024.202403903
Yanjun Liu, Jialin Zhang, Peiyi Wu
{"title":"Near-Frictionless Long-Distance Water Transport in Trees Enabled by Hierarchically Helical Molecular Pumps","authors":"Yanjun Liu, Jialin Zhang, Peiyi Wu","doi":"10.31635/ccschem.024.202403903","DOIUrl":"https://doi.org/10.31635/ccschem.024.202403903","url":null,"abstract":"The ascent of water in tall trees has fascinated scientists for over 130 years. However, the microscopic state and dynamic behavior of water within natural and undisturbed trees remain unknown. Here, we employ low-field nuclear magnetic resonance (NMR) to monitor the distribution and movement of water within a living tree in situ, uncovering a counterintuitive water transport process. The hierarchical walls of xylem vessels serve as the primary channels for continuous ascent of water, while the xylem vessels function more like a temporary water reservoir. The helical nanofibers within the vessel walls, which consist of series-wound crystalline and amorphous regions, create a helical Venturi molecular pump structure that efficiently draws water from the xylem vessel reservoir. Importantly, these helical nanofibers possess a semi-disordered surface embedded with a layer of solid-state water akin to a layer of ice. This self-lubricating layer of ice-like monolayer water, combined with the new “ground level” created by the helical arrangement of nanofibers, enables virtually frictionless long-distance transport of water under low negative pressure. Our findings challenge existing theories and offer valuable insights for developing biomimetic fiber pumps characterized by high efficiency and low energy consumption in fluid transportation.\u0000<figure><img alt=\"\" data-lg-src=\"/cms/asset/ec09e3da-db53-445f-a250-39ec461ce09a/keyimage.jpg\" data-src=\"/cms/asset/df24a2dd-2a6d-4c65-9ae0-15aa821f2146/keyimage.jpg\" src=\"/specs/ux3/releasedAssets/images/loader-7e60691fbe777356dc81ff6d223a82a6.gif\"/><ul>\u0000<li>Download figure</li>\u0000<li>Download PowerPoint</li>\u0000</ul>\u0000</figure>","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":null,"pages":null},"PeriodicalIF":11.2,"publicationDate":"2024-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140604067","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Electrosynthesis of the Nylon-6 Precursor from Nitrate and Cyclohexanone over a Rutile TiO2 Catalyst","authors":"Lan Luo, Lingxiu Li, Liang Xu, Yifan Yan, Shanshan Zhang, Hua Zhou, Zhenhua Li, Mingfei Shao, Xue Duan","doi":"10.31635/ccschem.024.202403988","DOIUrl":"https://doi.org/10.31635/ccschem.024.202403988","url":null,"abstract":"<p>Electrocatalytic reduction of nitrate (NO<sub>3</sub><sup>−</sup>) to valuable organonitrogen compounds beyond ammonia is a promising strategy for mitigating the human-caused unbalance of the global nitrogen cycle. Herein, we present an electrochemical strategy for synthesizing cyclohexanone oxime (CHO), an important feedstock in nylon-6 production through hydrogenative coupling of NO<sub>3</sub><sup>−</sup> and cyclohexanone (CYC) using a rutile titanium dioxide (R-TiO<sub>2</sub>) catalyst under ambient conditions. The CHO productivity achieved 127.3 μmol cm<sup>−2</sup> h<sup>−1</sup> with a high Faradaic efficiency (FE) of 68.2% at a current density of 30 mA cm<sup>−2</sup>. Moreover, the yield of CHO reached 98.2%. We demonstrated that the electrosynthesis of CHO operated through a tandem reaction mechanism involving the in situ generation of hydroxylamine (NH<sub>2</sub>OH) from NO<sub>3</sub><sup>−</sup> reduction, followed by a spontaneous nucleophilic addition–elimination reaction between NH<sub>2</sub>OH and CYC. Additionally, we revealed that R-TiO<sub>2</sub> exhibited a superior scaling relation with a high NH<sub>2</sub>OH generation rate and excellent CYC adsorption ability, which promoted CHO production. This electrochemical strategy was also effective for the synthesis of different oximes. Finally, we designed a coupling reaction system to realize the simultaneous production of CHO and CYC by combining cathodic NO<sub>3</sub><sup>−</sup> reduction and anodic cyclohexane oxidation, demonstrating a greener and more economical approach.</p>","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":null,"pages":null},"PeriodicalIF":11.2,"publicationDate":"2024-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140553430","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Cationic Spherical Polypeptides with Immunogenic Cell Death Inducing Activity for Oncolytic Immunotherapy","authors":"Zhihui Guo, Tianze Huang, Renyong Yin, Yongchang Tian, Pengqi Wan, Xuan Yi, Gao Li, Peng Zhang, Chunsheng Xiao, Xuesi Chen","doi":"10.31635/ccschem.024.202303793","DOIUrl":"https://doi.org/10.31635/ccschem.024.202303793","url":null,"abstract":"<p>Immunogenic cell death (ICD) has gained increasing attention due to its capacity to trigger anticancer immunity. Herein, we report a series of fabricated cationic spherical polypeptides (CSPs) designated CSP-0 to CSP-57, with oncolytic activity and ICD-inducing ability. CSP-57 exerted the optimal broad-spectrum and tumor-cell-selective cytotoxicity by disrupting cell membranes and inducing cell necrosis. Moreover, CSP-57 damaged mitochondrial membranes, thereby elevating intracellular levels of reactive oxygen species, leading to robust ICD of tumor cells featured by multiple damage-associated molecular patterns, including calreticulin, high-mobility group box 1, and adenosine triphosphate. In vivo anticancer activity determination results suggested that CSP-57 significantly delayed B16F10 tumor growth in mice by direct oncolysis and subsequent induction of ICD. The immunotherapeutic efficacy of CSP-57 was characterized by elevated ratios of cytotoxic T cells in tumors and spleens. Briefly, this work indicates that CSPs represent a promising strategy for oncolytic immunotherapy.</p>","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":null,"pages":null},"PeriodicalIF":11.2,"publicationDate":"2024-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140553312","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"A DNA-programmed Cargo Distributing System in Living Cells","authors":"Yuhan Wei, Yueyue Feng, Xiaoliang Chen, Wenhe Ma, Kaizhe Wang, Qian Li, Jiang Li, Lihua Wang, Chunhai Fan, Ying Zhu","doi":"10.31635/ccschem.024.202404080","DOIUrl":"https://doi.org/10.31635/ccschem.024.202404080","url":null,"abstract":"The functionalization of living cells, both internally and externally, transforming them into micromachines with specified functions, holds significant potential in fields such as biosensing, biocomputing, and intelligent theranostics. However, due to the complexity and dynamic nature of living cells, it remains challenging to allocate exogenous functional materials to specific locations within the cell or on its surface and maintain their positions stable for a reasonable period. Here, we devise a DNA-programmed cargo distributing system (DCD), capable of distributing functional modules to the cell membrane or within the cell as needed. This system includes an amphiphilic DNA structure for determining the destination of the cargo and a DNA connector carried on it for recognizing the DNA-encoded cargo. We test three different morphologies of amphiphilic DNA structures and find that their efficiencies in cell surface retention and cell internalization significantly varied, enabling the distribution of nanoparticle cargos on the cell membrane and within the cell in distinct proportions. Their positions can remain stable for at least 6 hours. Moreover, this allocation method shows specificity, which minimizes the deployment of mismatched cargo. This method provides new tools for the modular construction of cellular micromachines.\u0000<figure><img alt=\"\" data-lg-src=\"/cms/asset/00f94d08-4a6d-4e45-8bc5-ea2724a40021/keyimage.jpg\" data-src=\"/cms/asset/8d08d50e-b62a-40c8-a596-7bcde67e39b2/keyimage.jpg\" src=\"/specs/ux3/releasedAssets/images/loader-7e60691fbe777356dc81ff6d223a82a6.gif\"/><ul>\u0000<li>Download figure</li>\u0000<li>Download PowerPoint</li>\u0000</ul>\u0000</figure>","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":null,"pages":null},"PeriodicalIF":11.2,"publicationDate":"2024-04-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140603946","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
CCS ChemistryPub Date : 2024-04-11DOI: 10.31635/ccschem.024.202404104
Zekai Zhang, Qian He, Hengyi Wang, Changwei Liu, Hongchun Mu, Haiping Su, Xia Han, Honglai Liu, Cheng Lian
{"title":"An Ion-Channel-Reconstructed Water/Organic Amphiphilic Quasi-Solid-State Electrolyte for High-Voltage Energy Storage Devices","authors":"Zekai Zhang, Qian He, Hengyi Wang, Changwei Liu, Hongchun Mu, Haiping Su, Xia Han, Honglai Liu, Cheng Lian","doi":"10.31635/ccschem.024.202404104","DOIUrl":"https://doi.org/10.31635/ccschem.024.202404104","url":null,"abstract":"Quasi-solid-state electrolytes (QSSE) have garnered significant attention due to combining the dynamic properties of liquid electrolytes and the high safety of solid-state electrolytes. However, the limited electrochemical stability window (ESW) of liquid electrolytes and the low conductivity of the polymer matrix seriously constrain practical application. Herein, an ant-nest electrospun amphiphilic polyurethane-based gel electrolyte (eAPG) with hydrophilic ion channels in an organic polyurethane matrix was synthesized by swelling electrospun amphiphilic polyurethane (eAP) membrane in NaClO<sub>4</sub>-based trimethyl phosphate (TMP) aqueous solution. The dynamically reconstructed hydrophilic ion channels enhance the Na<sup>+</sup> transport rate five times compared to that in the polymer hydrophobic regions, which leads to a remarkable ion conductivity of 23.6 mS cm<sup>-1</sup>. The transport of free water in QSSEs via the <i>Grotthuss</i> mechanism is intimately associated with the ESW, where the eAP cross-linked network diminished the activity of free water, resulting in an increased ESW of 2.3V. Additionally, symmetric supercapacitors assembled by eAPG and activated carbon (AC) electrode exhibit 45.32 Wh kg<sup>-1</sup> at a power density of 0.933 kW kg<sup>-1</sup> with stable and long-term cycling. This rational electrolyte design strategy and remarkable electrochemical performance pave the way for the next generation of energy storage devices.\u0000<figure><img alt=\"\" data-lg-src=\"/cms/asset/aa52f114-65f4-43d8-9dbe-cdf0a04fbb8c/keyimage.jpg\" data-src=\"/cms/asset/f39a55e4-0b1f-4602-a377-e7303ced349e/keyimage.jpg\" src=\"/specs/ux3/releasedAssets/images/loader-7e60691fbe777356dc81ff6d223a82a6.gif\"/><ul>\u0000<li>Download figure</li>\u0000<li>Download PowerPoint</li>\u0000</ul>\u0000</figure>","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":null,"pages":null},"PeriodicalIF":11.2,"publicationDate":"2024-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140609844","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Regulating Mono/Binuclear Fe Species in Framework Al-Rich Zeolites for Efficient Low-Temperature Alkane Oxidation","authors":"Qiang Zhang, Jialiang Li, Guangyuan He, Junyan Li, Ziyi Chen, Qing Zhang, Chunyu Wang, Guodong Qi, Qiang Wang, Peng Zhang, Jun Xu, Osamu Terasaki, Donghai Mei, Zhongmin Liu, Jihong Yu","doi":"10.31635/ccschem.024.202404123","DOIUrl":"https://doi.org/10.31635/ccschem.024.202404123","url":null,"abstract":"Zeolite-encapsulated extra-framework mono/binuclear Fe<sup>3+</sup> species present higher catalytic activities compared to clusters and nanoparticles for direct low-temperature alkane oxidation. However, the fine control of mono/binuclear Fe<sup>3+</sup> in zeolites is challenging and the reaction mechanism of low-temperature alkane oxidation remains not clearly identified. Different from previous impregnation and ion-exchange methods generally generating clusters/nanoparticles, here we developed an efficient amino acid-assisted one-pot hydrothermal synthesis strategy for in situ incorporating mono/binuclear Fe<sup>3=</sup> species into framework Al-rich ZSM-5 zeolites. The high framework Al content (Si/Al=9) provided sufficient negatively-charged sites to anchor mono/binuclear Fe<sup>3+</sup> (Fe loading=0.44~0.90 wt%). The as-prepared 0.44Fe@Z-L<sub>0.3</sub>H<sub>6</sub>-9 catalyst exhibited superior catalytic properties for selective oxidation of both methane and ethane in the H<sub>2</sub>O<sub>2</sub> solution at 50 °C, presenting a top-level catalytic performance among various heterogeneous/homogeneous catalysts. Combining advanced characterizations and density functional theory calculations, the complex reaction networks for methane and ethane conversions into C1/C2 oxygenates over mononuclear and binuclear Fe<sup>3+</sup>, for the first time, were mapped out. The mononuclear Fe<sup>3+</sup> was found more active than binuclear Fe<sup>3+</sup> for both methane and ethane conversions. This work not only provides a whole picture on low-temperature alkane oxidation mechanisms but also guides the rational design of high-performance catalysts for C−H bond activation and beyond.\u0000<figure><img alt=\"\" data-lg-src=\"/cms/asset/5089ba4d-1638-4cd0-a1d2-d75a33f61caa/keyimage.jpg\" data-src=\"/cms/asset/39784551-9e90-43f1-91c7-78f75456622b/keyimage.jpg\" src=\"/specs/ux3/releasedAssets/images/loader-7e60691fbe777356dc81ff6d223a82a6.gif\"/><ul>\u0000<li>Download figure</li>\u0000<li>Download PowerPoint</li>\u0000</ul>\u0000</figure>","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":null,"pages":null},"PeriodicalIF":11.2,"publicationDate":"2024-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140609366","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
CCS ChemistryPub Date : 2024-04-11DOI: 10.31635/ccschem.024.202404292
Aimin Li, Yuanchu Liu, Ke Luo, Qing He
{"title":"CO2 Capture in Liquid Phase and Room–Temperature Release and Concentration Using Mechanical Power","authors":"Aimin Li, Yuanchu Liu, Ke Luo, Qing He","doi":"10.31635/ccschem.024.202404292","DOIUrl":"https://doi.org/10.31635/ccschem.024.202404292","url":null,"abstract":"Development of advanced materials with high CO<sub>2</sub> capture capacity and, <i>inter alia</i>, superior regenerability with low energy consumption (low–temperature CO<sub>2</sub> release) remains highly desired yet challenging. Herein, we firstly report the precipitation–involved CO<sub>2</sub> capture from ultradilute sources (e.g., exhaled gas and indoor air) and the reversible room–temperature CO<sub>2</sub> release accelerated by mechanical power using a covalent organic superphane cage. This superphane based operating system enables CO<sub>2</sub> in ultradilute gas (< 6%) to be concentrated up to 83%. As inferred from the control experiments and theoretical calculations, this proof–of–concept CO<sub>2</sub> capture and concentration system with mechanical power–triggered CO<sub>2</sub> release by the discrete organic cage could be rationalized by the formation of a six–membered ring transition state with relatively low energy barrier during the process of the adsorption and desorption of CO<sub>2</sub> on the cage surface, along with the precipitation involved phase change.\u0000<figure><img alt=\"\" data-lg-src=\"/cms/asset/7e6328b1-9517-4a75-9049-1c025baa2278/keyimage.jpg\" data-src=\"/cms/asset/41fb7540-b7d1-4c94-b3bb-760edc1b5ab8/keyimage.jpg\" src=\"/specs/ux3/releasedAssets/images/loader-7e60691fbe777356dc81ff6d223a82a6.gif\"/><ul>\u0000<li>Download figure</li>\u0000<li>Download PowerPoint</li>\u0000</ul>\u0000</figure>","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":null,"pages":null},"PeriodicalIF":11.2,"publicationDate":"2024-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140595934","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
CCS ChemistryPub Date : 2024-04-11DOI: 10.31635/ccschem.024.202404120
Yuxiang Huang, Yuchen Ji, Guorui Zheng, Hongbin Cao, Haoyu Xue, Xiangming Yao, Lu Wang, Shiming Chen, Zuwei Yin, Feng Pan, Luyi Yang
{"title":"Tailored Interphases Construction for Enhanced Si Anode and Ni-Rich Cathode Performance in Lithium-Ion Batteries","authors":"Yuxiang Huang, Yuchen Ji, Guorui Zheng, Hongbin Cao, Haoyu Xue, Xiangming Yao, Lu Wang, Shiming Chen, Zuwei Yin, Feng Pan, Luyi Yang","doi":"10.31635/ccschem.024.202404120","DOIUrl":"https://doi.org/10.31635/ccschem.024.202404120","url":null,"abstract":"As promising candidates for high-energy-density lithium-ion batteries, both silicon (Si) anodes and nickel-rich cathodes face significant challenges due to structural instability arising from interphases. In this study, we introduce tetravinylsilane (TVSi) as a multifunctional electrolyte additive to engineer tailored interphases simultaneously on Si anode and LiNi<sub>0.92</sub>Mn<sub>0.05</sub>Co<sub>0.03</sub>O<sub>2</sub> cathode, thereby enhancing their electrochemical performance. On one front, TVSi undergoes polymerization, leading to the formation of a composite solid electrolyte interphase (SEI) with an interpenetrating network structure on the Si surface. This SEI effectively accommodates the volume changes during cycling, inhibiting SEI growth and thereby preserving the capacity. On the other front, the TVSi-induced cathode-electrolyte interphase (CEI) exhibits a dense structure comprising a chemically bonded silicate-silane polymer. This CEI effectively mitigates transition metal dissolution by scavenging hydrofluoric acid and reduces irreversible phase transitions by minimizing side reactions. As a result of the enhanced interfacial stability achieved on both electrodes, TVSi enables improved performance in full cells with a LiNi<sub>0.92</sub>Mn<sub>0.05</sub>Co<sub>0.03</sub>O<sub>2</sub> cathode paired with a silicon anode. This multifunctional additive strategy offers a novel perspective on additive design for high-energy-density lithium-ion batteries, showcasing its potential for advancing battery technology.\u0000<figure><img alt=\"\" data-lg-src=\"/cms/asset/bd2b489e-0c04-43e0-bc57-ca8688d8e502/keyimage.jpg\" data-src=\"/cms/asset/809c828a-9af8-4417-bd98-a84ceb96f17e/keyimage.jpg\" src=\"/specs/ux3/releasedAssets/images/loader-7e60691fbe777356dc81ff6d223a82a6.gif\"/><ul>\u0000<li>Download figure</li>\u0000<li>Download PowerPoint</li>\u0000</ul>\u0000</figure>","PeriodicalId":9810,"journal":{"name":"CCS Chemistry","volume":null,"pages":null},"PeriodicalIF":11.2,"publicationDate":"2024-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140609512","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}